Abstract

Abstract. Regional transport and heterogeneous reactions have been shown to play crucial roles in haze formation over a megacity cluster centered on Beijing. In this study, the updated Nested Air Quality Prediction Model System (NAQPMS) and the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model were employed to investigate the evolution of aerosols – in terms of the number concentration, size distribution, and degree of aging – in Beijing during six haze episodes between 15 November and 15 December 2016, as part of the Air Pollution and Human Health–Beijing (APHH-Beijing) winter campaign of 2016. The model exhibited reasonable performance not only with respect to mass concentrations of PM2.5 and its components in Beijing but also regarding the number concentration, size distribution, and degree of aging. We revealed that regional transport played a non-negligible role in haze episodes, with contributions of 14 %–31 % to the surface PM2.5 mass concentration. The contribution of regional transport to secondary inorganic aerosols was larger than that to primary aerosols (30 %–63 % and 3 %–12 %, respectively). The chemical transformation of SO2 along the transport pathway from source regions to Beijing was the major source of SO42-. We also found that sulfate formed outside Beijing from SO2 emitted in Beijing; this sulfate was then blown back to Beijing and considerably influenced haze formation. Along the transport pathway, aerosols underwent aging, which altered the mass ratio of the coating of black carbon to black carbon (RBC) and the size distribution of number concentrations. During the episodes, the geometric mean diameter (GMD) increased from less than 100 nm at the initial site to approximately 120 nm at the final site (Beijing), and the RBC increased from 2–4 to 4–8. During haze episodes with high humidity, the average contributions of gas and aqueous chemistry, heterogeneous chemistry, and primary emission to sulfate were comparable. However, their relative contributions varied with pollution levels. Primary emissions had the greatest impact under light to moderate pollution levels, whereas heterogeneous chemistry had a stronger effect under high pollution levels.

Highlights

  • In past decades, a megacity cluster in China that is centered on Beijing and includes 28 cities (272 500 km2, with a population of 191.7 million people) has experienced frequent severe and persistent haze episodes (Zhao et al, 2013; Sun et al, 2014, 2016)

  • The PM2.5 mass concentrations ranged from 75 to 115 μg m−3, indicating a light pollution level according to the Technical Regulation on Ambient Air Quality Index

  • In contrast to PIA, the secondary inorganic aerosol (SIA) contribution was dominated by regional transport of emissions from other cities (50 %–87 %)

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Summary

Introduction

A megacity cluster in China that is centered on Beijing and includes 28 cities (272 500 km, with a population of 191.7 million people) has experienced frequent severe and persistent haze episodes (Zhao et al, 2013; Sun et al, 2014, 2016). Using a ceilometer and in situ observation data, Zhu et al (2016) and Ma et al (2017) further proposed that regional transport was the major cause of the initial haze stage and that local chemistry, heterogeneous chemistry, dominated the subsequent later rise in Beijing. This result differs from the findings of modeling studies We believe that this study will help to understand the causes of haze in this megacity cluster

Model description
Model configuration
Emission inventory
Observations
Model validation
Meteorology
Results and discussion
The impact of regional transport of sulfate and its precursors in Beijing
Evolution of aerosol properties in Beijing during haze episodes
Impact of heterogeneous chemistry on sulfate mass concentration
Conclusions
Full Text
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